Otherwise, Jorge Ben made several great albums, the best of which are probably A Tábua de Esmeralda (1974) and África Brasil (1976). His mid-60's samba albums are also great fun (Samba Esquema Novo  probably the most consistent).
Also, as a big fan of 1966-71 Chico Buarque, I'd caution that not understanding Portuguese takes more away from his work than any of the other artists mentioned, though it's probably still good even if jibberish to you.
Finally, can't leave out Elis & Tom (1974), quite possibly the best bossa nova album ever.
In Spanish, I'm not as knowledgeable, but Café Tacuba's Re (1994) is a definite must, esp. for anyone who likes themselves some Ween (i.e. shockingly consistent and well-done genre send-ups).